Origin of weak magnetism in compounds with cubic laves structure.

The origin of the weak itinerant magnetism in materials such as TiBe2 and ZrZn2 is investigated. The huge peak in the density of states at the Fermi energy is attributed to a special symmetry of the C15 structure: no crystal field splitting of the d levels occurs in the case of coordination by spherical ligands. Crystal field splitting is also investigated for the f orbitals in C15 structures such as PuZn2 and ThMg2. It is observed that the situation in f levels is more complicated than the d levels because the characteristics of the crystal field splitting for f levels does not only depend on the the local point symmetry of the compounds.

The electronic structure of organic-inorganic hybrid compounds: (NH4)2CuCl4, (CH3NH3)2CuCl4 and (C2H5NH3)2CuCl4.

Hybrid organic-inorganic compounds are an intriguing class of materials that have been experimentally studied over the past few years because of a potential broad range of applications. The electronic and magnetic properties of three organic-inorganic hybrid compounds with compositions (NH4)2CuCl4, (CH3NH3)2CuCl4 and (C2H5NH3)2CuCl4 are investigated for the first time with density functional theory plus on-site Coulomb interaction. A strong Coulomb interaction on the copper causes a relatively weak exchange coupling within the layers of the octahedral network, in good agreement with experiment. The character of the exchange interaction (responsible for magnetic behavior) is analyzed. The calculations reveal that (C2H5NH3)2CuCl4 has the strongest Jahn-Teller (JT) distortion in comparison with the two other compounds. The easy axis of magnetization is investigated, showing a weak anisotropic interaction between inter-layer Cu(2+) ions in the (C2H5NH3)2CuCl4 structure. Orbital ordering is concluded from our partial density of states calculations: a cooperation of the JT distortion with an antiferro-distortive pattern.

Intrinsic defects and dopants in LiNH2: a first-principles study.

The lithium amide (LiNH(2)) + lithium hydride (LiH) system is one of the most attractive light-weight materials options for hydrogen storage. Its dehydrogenation involves mass transport in the bulk (amide) crystal through lattice defects. We present a first-principles study of native point defects and dopants in LiNH(2) using density functional theory. We find that both Li-related defects (the positive interstitial Li(i)(+) and the negative vacancy V(Li)(-)) and H-related defects (H(i)(+) and V(H)(-)) are charged. Li-related defects are most abundant. Having diffusion barriers of 0.3-0.5 eV, they diffuse rapidly at moderate temperatures. V(H)(-) corresponds to the [NH](2-) ion. It is the dominant species available for proton transport with a diffusion barrier of ∼0.7 eV. The equilibrium concentration of H(i)(+), which corresponds to the NH(3) molecule, is negligible in bulk LiNH(2). Dopants such as Ti and Sc do not affect the concentration of intrinsic defects, whereas Mg and Ca can alter it by a moderate amount. Ti and Mg are easily incorporated into the LiNH(2) lattice, which may affect the crystal morphology on the nano-scale.

Spin tunneling in junctions with disordered ferromagnets.

We provide compelling evidence to establish that, contrary to one's elementary guess, the tunneling spin polarization (TSP) of amorphous CoFeB is larger than that of fcc CoFeB. First-principles atomic and electronic structure calculations reveal striking agreement between the measured TSP and the predicted s-electron spin polarization. Given the disordered structure of the ternary alloy, not only do these results strongly endorse our communal understanding of tunneling through AlO(x), but they also portray the key concepts that demand primary consideration in such complex systems.

Electronic band structure of tetracene-TCNQ and perylene-TCNQ compounds.

The relationship between the crystal structures, band structures, and electronic properties of acene-TCNQ complexes has been investigated. We focus on the newly synthesized crystals of the charge-transfer salt tetracene-TCNQ and similar to it perylene-TCNQ, potentially interesting for realization of ambipolar transport. The band structures were calculated from first principles using density-functional theory (DFT). Despite the similarity in the crystal structures of the acene-TCNQ complexes studied here, the band structures are very different. Hole and electron transport properties are predicted to be equally good in perylene-TCNQ, in contrast to the tetracene-TCNQ, which has good transport properties for electrons only. The estimated degree of charge transfer for tetracene-TCNQ is 0.13e and for perylene-TCNQ 0.46e.

Optimizing performance of half-metals at finite temperature.

Several aspects of half-metallic magnetism at finite temperature are discussed. Since NiMnSb is the simplest half-metal and the longest known it will be used as an example. Also it is a half-metal with remarkable little on-site Coulomb repulsion. Consequently it is a half-metal that is not notably corrupted by non-quasiparticle states. There exists an anomaly at 90 K, described before, that will be shown to be unrelated to the position of the Fermi level in the bandgap. Several substitutions are investigated that could shed some light on the origin of the transition. The calculated phonon spectrum is compared with experimental neutron scattering data. Finally, the spin-polarization of interfaces of NiMnSb with the transition metal based non-magnetic semiconductors NiTiSn and CoTiSb is investigated and the electronic structure of an infinite two-dimensional array of NiMnSb quantum dots embedded in NiScSb is reported.

Ab initio and work function and surface energy anisotropy of LaB6.

Lanthanum hexaboride is one of the cathode materials most used in high-power electronics technology, but the many experimental results do not provide a consistent picture of the surface properties. Therefore, we report the first ab initio calculations of the work functions and surface energies of the (001), (011), (111), (112), and (012) surfaces by considering the different surface terminations and structural relaxation. Either the (111)B- or the (001)La-terminated surface is the most stable, depending on La chemical potential. The work function of the latter is the lowest (2.07 eV) of the surfaces considered. Both the work function and surface energy decrease further when surface La is replaced by Ba and become, respectively, 1.43 and 7.7 eV/nm(2) at the chemical potentials of elemental lanthanum and barium bulk. These results compare favorably with previous work on the intermetallics BaAl(4), CaAl(4), and BaAuIn(3). Their most stable surfaces possess the lowest work function. Now, we study a compound with a decidedly different crystal type and with its constituting elements from column 3 of the periodic table, of which one is nonmetallic.